Self-assembled Hydrogel Fiber Bundles from Oppositely Charged Polyelectrolytes Mimic Micro-/nanoscale Hierarchy of Collagen. Academic Article uri icon


  • Fiber bundles are present in many tissues throughout the body. In most cases, collagen subunits spontaneously self-assemble into a fibrilar structure that provides ductility to bone and constitutes the basis of muscle contraction. Translating these natural architectural features into a biomimetic scaffold still remains a great challenge. Here, we propose a simple strategy to engineer biomimetic fiber bundles that replicate the self-assembly and hierarchy of natural collagen fibers. The electrostatic interaction of methacrylated gellan gum (MeGG) with a countercharged chitosan (CHT) polymer led to the complexation of the polyelectrolytes. When directed through a polydimethylsiloxane (PDMS) channel, the polyelectrolytes formed a hierarchical fibrous hydrogel demonstrating nano-scale periodic light/dark bands similar to D-periodic bands in native collagen and aligned parallel fibrils at micro-scale. Importantly, collagen-mimicking hydrogel fibers exhibited robust mechanical properties (MPa scale) at a single fiber bundle level and enabled encapsulation of cells inside the fibers under cell-friendly mild conditions. Presence of carboxyl- (in gellan gum) or amino- (in chitosan) functionalities further enabled controlled peptide functionalization such as RGD for biochemical mimicry (cell adhesion sites) of native collagen. This biomimetic aligned fibrous hydrogel system can potentially be used as a scaffold for tissue engineering as well as a drug/gene delivery vehicle.

published proceedings

  • Adv Funct Mater

altmetric score

  • 1.25

author list (cited authors)

  • Sant, S., Coutinho, D. F., Gaharwar, A. K., Neves, N. M., Reis, R. L., Gomes, M. E., & Khademhosseini, A.

citation count

  • 54

complete list of authors

  • Sant, Shilpa||Coutinho, Daniela F||Gaharwar, Akhilesh K||Neves, Nuno M||Reis, Rui L||Gomes, Manuela E||Khademhosseini, Ali

publication date

  • September 2017